![]() Intriguingly, benefiting from the quantum confinement effects in the out-of-plane direction, two-dimensional (2D) materials are highly promising for high-performance optoelectronic devices, which are compatible with current thin-film microfabrication techniques appropriately. However, the complexity in manipulation and poor uniformity of 1D/QD materials impede their realistic applications. Until now, by employing quantum dots (QDs) and one-dimensional (1D) semiconducting nanostructures of ZrS 2, CdS, and ZnO as sensitizers, ,, high-performance photodetectors (PDs) have been demonstrated. The charge separation promoted by surface states is considered to be responsible for the prolonged photocarrier lifetime, resulting in a high photocurrent gain. Nanomaterials are gaining intense interest in photodetection due to their large surface-to-volume ratios and low dimensions, which can yield higher light sensitivity than their bulk counterparts. We anticipate that these results are generalizable to other layer semiconductors as well. Our findings revealed a pathway for the development of high-performance PDs based on 2D MoSe 2 that are inexpensive, large area, and suitable for mass production and contribute to a deep understanding of the photoconductivity mechanisms in atomically thin MoSe 2. Additionally, the ultrahigh photoresponsivity and low dark current that originated from Schottky barrier resulted in a record-high specific detectivity of up to 2×10 13 Jones for 2D MoSe 2/MoS 2 PDs. A fast response time of 22 ms was observed and attributed to effective nonequilibrium carrier recombination. We extracted an ultrahigh photoresponsivity approaching 101 A/W with concomitantly high external quantum efficiency up to 19,668% due to the produced gain arising from the holes trapped at the metal/MoSe 2 interface, the band tail state contribution, and the photogating effect. Moreover, a metal-semiconductor-metal photodetector (PD) was fabricated and investigated systematically. The reduction of MoO 3 was found indispensable for the successful synthesis of MoSe 2 films due to the low vaporization temperature. In this work, we reported a method involving atomic layer deposition and a chemical vapor deposition chamber to produce few-layer 2H-MoSe 2 thin films with wafer-level uniformity. However, the lack of efficient and stable approaches to synthesize large-area thin films with excellent uniformity hinders their realistic applications. The unique structural and physical properties of two-dimensional (2D) atomic layer semiconductors render them promising candidates for electronic or optoelectronic devices. ![]()
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